Non-local linear-response functions for thermal transport computed with equilibrium molecular-dynamics simulation

TL;DR

This paper introduces a method to compute non-local thermal response functions using equilibrium molecular dynamics, revealing the transition from ballistic to diffusive heat transport in crystals.

Contribution

The study develops a novel approach to calculate linear-response functions for thermal transport, capturing non-local effects and partial ballistic behavior in molecular dynamics simulations.

Findings

Transport is ballistic at low temperatures and short scales.

At higher temperatures and longer scales, transport aligns with Fourier's law.

Effective thermal conductivity can be extracted in the ballistic regime.

Abstract

We establish an approach to compute linear-response functions to elucidate heat waves and non-local thermal transport. The theory is able to describe the response of a system to external heat sources that are nonuniform in space and time. The response functions are computed using equilibrium molecular-dynamics simulations of an Ar crystal modeled using the standard Lennard-Jones potential. It is shown that for low temperatures and short length scales, transport can be partially or even completely ballistic, with the response primarily limited by the group velocity of lattice waves. By contrast, at longer length scales and higher temperatures, the response functions correspond more closely to diffusive transport characteristic of Fourier's law. It is also shown how the effective thermal conductivity can be determined in a partially-ballistic regime. The results demonstrate the known reduction in the effective thermal conductivity observed when system dimensions are smaller than the mean-free path for lattice waves. Finally, we show how determination of the relevant response functions can be used to model heating of a crystal without requiring additional atomic-scale simulations. Differences between computed results and predictions from Fourier's law represent wave-like, partially-ballistic transport.